Comparison of behaviour of rare earth containing catalysts in the oxidative dehydrogenation of ethane

被引:39
作者
Ciambelli, P
Lisi, L
Pirone, R
Ruoppolo, G
Russo, G
机构
[1] Univ Salerno, Dipartimento Ingn Chim & Alimentare, I-84084 Salerno, Italy
[2] CNR, Ist Ric Combust, I-80125 Naples, Italy
[3] Univ Naples Federico II, Dipartimento Ingn Chim, Naples, Italy
关键词
rare earth catalysts; oxidative dehydrogenation; ethane;
D O I
10.1016/S0920-5861(00)00391-6
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Catalyst promotion by addition of either La and Sm to MgO or Na aluminate to Sm2O3 and La2O3 has been investigated for the oxidative dehydrogenation of ethane in the temperature range 550-700 degrees C. With all unpromoted and promoted catalysts, the selectivity to ethylene is strongly enhanced by the temperature, the highest values being obtained at 700 degrees C. Sm2O3 is the most active among the bulk oxides. while samarium addition to MgO results in higher surface area, but does not enhance the catalytic activity. Ethylene productivity on La2O3 promoted MgO samples is higher than with pure La2O3, Sm2O3 and MgO, not only due ro the stabilising effect of La on MgO surface area, but also due to a higher intrinsic activity. With both bulk oxides and rare earth promoted MgO, the selectivity to ethylene strongly increases by decreasing the O-2/C2H6 feed ratio, while it is quite unaffected by ethane conversion and catalyst composition. in agreement with the hypothesis that the main role of catalyst in the experimental conditions investigated is to produce ethyl radicals which are converted in the gas phase to CO and C2H4. When La2O3 is modified by the addition of sodium aluminate the catalytic behaviour significantly changes, Likely due to a different, mostly heterogeneous reaction mechanism. On aluminate promoted lanthana, ethane is converted to ethylene with higher yields which do not depend on the feed ratio. Moreover. only CO2 is produced as by-product, the formation of CO being quite negligible. (C) 2000 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:317 / 323
页数:7
相关论文
共 17 条
[1]   HOMOGENEOUS AND HETEROGENEOUS CONTRIBUTIONS TO THE CATALYTIC OXIDATIVE DEHYDROGENATION OF ETHANE [J].
BURCH, R ;
CRABB, EM .
APPLIED CATALYSIS A-GENERAL, 1993, 97 (01) :49-65
[2]   COMPARATIVE-STUDY OF CATALYSTS FOR THE OXIDATIVE COUPLING OF METHANE [J].
BURCH, R ;
SQUIRE, GD ;
TSANG, SC .
APPLIED CATALYSIS, 1988, 43 (01) :105-116
[3]   INVESTIGATION OF THE PARTIAL OXIDATION OF HYDROCARBONS ON METHANE COUPLING CATALYSTS [J].
BURCH, R ;
TSANG, SC .
APPLIED CATALYSIS, 1990, 65 (02) :259-280
[4]   TRANSIENT STUDIES ON REACTION STEPS IN THE OXIDATIVE COUPLING OF METHANE OVER CATALYTIC SURFACES OF MGO AND SM2O3 [J].
BUYEVSKAYA, OV ;
ROTHAEMEL, M ;
ZANTHOFF, HW ;
BAERNS, M .
JOURNAL OF CATALYSIS, 1994, 146 (02) :346-357
[5]   THE OXIDATIVE DEHYDROGENATION OF ETHANE AND PROPANE AS AN ALTERNATIVE WAY FOR THE PRODUCTION OF LIGHT OLEFINS [J].
CAVANI, F ;
TRIFIRO, F .
CATALYSIS TODAY, 1995, 24 (03) :307-313
[6]   Pulse reactions of methane, ethane and ethylene over Li-, La- and Sm-promoted MgO catalysts in the presence and absence of free oxygen [J].
Choudhary, VR ;
Rane, VH ;
Chaudhari, ST .
REACTION KINETICS AND CATALYSIS LETTERS, 1998, 63 (02) :371-377
[7]   Surface properties of rare earth promoted MgO catalysts and their catalytic activity/selectivity in oxidative coupling of methane [J].
Choudhary, VR ;
Rane, VH ;
Chaudhari, ST .
APPLIED CATALYSIS A-GENERAL, 1997, 158 (1-2) :121-136
[8]  
CIAMBELLI P, 1997, STUD SURF SCI CATAL, V110, P287
[9]   Oxidative Coupling of Methane on Sodium Aluminate- and Magnesium Oxide- supported Samarium Oxide [J].
Hamid, H. B. A. ;
Moyes, R. B. .
CATALYSIS TODAY, 1991, 10 (03) :267-274
[10]   The oxidative dehydrogenation of ethane over alkali-doped lanthanum-calcium oxide catalysts [J].
Ji, L ;
Liu, JS ;
Chen, XC ;
Li, M .
CATALYSIS LETTERS, 1996, 39 (3-4) :247-252